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1.
• UV/O3 process had higher TAIC mineralization rate than O3 process. • Four possible degradation pathways were proposed during TAIC degradation. • pH impacted oxidation processes with pH of 9 achieving maximum efficiency. • CO32– negatively impacted TAIC degradation while HCO3 not. • Cl can be radicals scavenger only at high concentration (over 500 mg/L Cl). Triallyl isocyanurate (TAIC, C12H15N3O3) has featured in wastewater treatment as a refractory organic compound due to the significant production capability and negative environmental impact. TAIC degradation was enhanced when an ozone(O3)/ultraviolet(UV) process was applied compared with the application of an independent O3 process. Although 99% of TAIC could be degraded in 5 min during both processes, the O3/UV process had a 70%mineralization rate that was much higher than that of the independent O3 process (9%) in 30 min. Four possible degradation pathways were proposed based on the organic compounds of intermediate products identified during TAIC degradation through the application of independent O3 and O3/UV processes. pH impacted both the direct and indirect oxidation processes. Acidic and alkaline conditions preferred direct and indirect reactions respectively, with a pH of 9 achieving maximum Total Organic Carbon (TOC) removal. Both CO32– and HCO3 decreased TOC removal, however only CO32– negatively impacted TAIC degradation. Effects of Cl as a radical scavenger became more marked only at high concentrations (over 500 mg/L Cl). Particulate and suspended matter could hinder the transmission of ultraviolet light and reduce the production of HO· accordingly.  相似文献   

2.
• Regulation of redox conditions promotes the generation of free radicals on HM. • HM-PFRs can be fractionated into active and inactive types depending on stability. • The newly produced PFRs readily release electrons to oxygen and generate ROS. • PFR-induced ROS mediate the transformation of organic contaminants adsorbed on HM. The role of humic substance-associated persistent free radicals (PFRs) in the fate of organic contaminants under various redox conditions remains unknown. This study examined the characterization of original metal-free peat humin (HM), and HM treated with varying concentrations of H2O2 and L-ascorbic acid (VC) (assigned as H2O2-HM and VC-HM). The concentration of PFRs in HM increased with the addition of VC/H2O2 at concentrations less than 0.08 M. The evolution of PFRs in HM under different environmental conditions (e.g., oxic/anoxic and humidity) was investigated. Two types of PFRs were detected in HM: a relatively stable radical existed in the original sample, and the other type, which was generated by redox treatments, was relatively unstable. The spin densities of VC/H2O2-HM readily returned to the original value under relatively high humidity and oxic conditions. During this process, the HM-associated “unstable” free radicals released an electron to O2, inducing the formation of reactive oxygen species (ROS, i.e., OH and O2). The generated ROS promoted the degradation of polycyclic aromatic hydrocarbons based on the radical quenching measurements. The transformation rates followed the order naphthalene>phenanthrene>anthracene>benzo[a]pyrene. Our results provide valuable insight into the HM-induced transformation of organic contaminants under natural conditions.  相似文献   

3.
• Bi doping in TiO2 enhanced the separation of photo-generated electron-hole. • The performance of photocatalytic degradation of MC-LR was improved. • Coexisting substances have no influence on algal removal performance. • The key reactive oxygen species were h+ and OH in the photocatalytic process. The increase in occurrence and severity of cyanobacteria blooms is causing increasing concern; moreover, human and animal health is affected by the toxic effects of Microcystin-LR released into the water. In this paper, a floating photocatalyst for the photocatalytic inactivation of the harmful algae Microcystis aeruginosa (M. aeruginosa) was prepared using a simple sol-gel method, i.e., coating g-C3N4 coupled with Bi-doped TiO2 on Al2O3-modified expanded perlite (CBTA for short). The impact of different molar ratios of Bi/Ti on CBTA was considered. The results indicated that Bi doping in TiO2 inhibited photogenerated electron-hole pair recombination. With 6 h of visible light illumination, 75.9% of M. aeruginosa (initial concentration= 2.7 × 106 cells/L) and 83.7% of Microcystin-LR (initial concentration= 100 μg/L) could be removed with the addition of 2 g/L CBTA-1% (i.e., Bi/Ti molar ratio= 1%). The key reactive oxygen species (ROSs) in the photocatalytic inactivation process are h+ and OH. The induction of the Bi4+/Bi3+ species by the incorporation of Bi could narrow the bandgap of TiO2, trap electrons, and enhance the stability of CBTA-1% in the solutions with coexisting environmental substances.  相似文献   

4.
• Humification evolution was identified with non-destructive characterization method. • Humification process from precursors to fulvic and humic acid was confirmed. • MnO2 alone had limited oxidation ability to form HA. • MnO2 played a key role as a catalyst to transform FA to HA in the presence of O2. • MnO2 could affect the structure of the humification products. Abiotic humification is important in the formation and evolution of organic matter in soil and compost maturing processes. However, the roles of metal oxides in abiotic humification reactions under micro-aerobic remain ambiguous. The aim of this study was to use non-destructive measurement methods to investigate the role of MnO2 in the evolution of humic substances (HSs) during oxidative polymerization of polyphenol-amino acid. Our results suggested a synergistic effect between MnO2 and O2 in promoting the polymerization reaction and identified that MnO2 alone had a limited ability in accelerating the transformation of fulvic acid (FA) to humic acid (HA), whereas O2 was the key factor in the process. Two-dimensional correlation spectroscopy (2D-COS) showed that the evolution in the UV-vis spectra followed the order of 475–525 nm>300–400 nm>240–280 nm in the humification process, indicating the formation of simple organic matter followed by FA and then HA. 13C nuclear magnetic resonance (13C NMR) analysis revealed that the products under both air and N2 conditions in the presence of MnO2 had greater amounts of aromatic-C than in the absence of MnO2, demonstrating that MnO2 affected the structure of the humification products. The results of this study provided new insights into the theory of abiotic humification.  相似文献   

5.
• Annual AOCs in MBR effluents were stable with small increase in warmer seasons. • Significant increase in AOC levels of tertiary effluents were observed. • Coagulation in prior to ozonation can reduce AOC formation in tertiary treatment. • ∆UV254 and SUVA can be surrogates to predict the AOC changes during ozonation. As water reuse development has increased, biological stability issues associated with reclaimed water have gained attention. This study evaluated assimilable organic carbon (AOC) in effluents from a full-scale membrane biological reactor (MBR) plant and found that they were generally stable over one year (125–216 µg/L), with slight increases in warmer seasons. After additional tertiary treatments, the largest increases in absolute and specific AOCs were detected during ozonation, followed by coagulation-ozonation and coagulation. Moreover, UV254 absorbance is known to be an effective surrogate to predict the AOC changes during ozonation. Applying coagulation prior to ozonation of MBR effluents for removal of large molecules was found to reduce the AOC formation compared with ozonation treatment alone. Finally, the results revealed that attention should be paid to seasonal variations in influent and organic fraction changes during treatment to enable sustainable water reuse.  相似文献   

6.
• N-Cl-DCAM, an emerging N-DBP in drinking water was investigated. • A new BAC has a better removal efficiency for N-Cl-DCAM precursors than an old BAC. • N-Cl-DCAM precursors are more of low molecular weight and non-polar. • Adsorption of GAC plays a major role in removal of N-Cl-DCAM precursors by an O3-BAC. N-chloro-2,2-dichloroacetamide (N-Cl-DCAM) is an emerging nitrogenous disinfection by-product (N-DBP) which can occur in drinking water. In this study, an analytical method based on liquid chromatography with tandem mass spectrometry (LC-MS/MS) was developed to validate the concentration of N-Cl-DCAM, which was found to be 1.5 mg/L in the effluent of a waterworks receiving raw water from Taihu Lake, China. The changes of N-Cl-DCAM formation potential (N-Cl-DCAMFP) in the drinking water treatment process and the removal efficiency of its precursors in each unit were evaluated. Non-polar organics accounted for the majority of N-Cl-DCAM precursors, accounting for 70% of the N-Cl-DCAM FP. The effect of conventional water treatment processes on the removal of N-Cl-DCAM precursors was found to be unsatisfactory due to their poor performance in the removal of low molecular weight (MW) or non-polar organics. In the ozonation integrated with biological activated carbon (O3-BAC) process, the ozonation had little influence on the decrease of N-Cl-DCAM FP. The removal efficiency of precursors by a new BAC filter, in which the granular activated carbon (GAC) had only been used for four months was higher than that achieved by an old BAC filter in which the GAC had been used for two years. The different removal efficiencies of precursors were mainly due to the different adsorption capacities of GAC for individual precursors. Low MW or non-polar organics were predominantly removed by GAC, rather than biodegradation by microorganisms attached to GAC particles.  相似文献   

7.
• Complete CT degradation was achieved by employing HA to CP/Fe(II)/FA process. • Quantitative detection of Fe(II) regeneration and HO• production was investigated. • Benzoic acid outcompeted FA for the reaction with HO•. • CO2 was the dominant reductive radical for CT removal. • Effects of solution matrix on CT removal were conducted. Hydroxyl radicals (HO•) show low reactivity with perchlorinated hydrocarbons, such as carbon tetrachloride (CT), in conventional Fenton reactions, therefore, the generation of reductive radicals has attracted increasing attention. This study investigated the enhancement of CT degradation by the synergistic effects of hydroxylamine (HA) and formic acid (FA) (initial [CT] = 0.13 mmol/L) in a Fe(II) activated calcium peroxide (CP) Fenton process. CT degradation increased from 56.6% to 99.9% with the addition of 0.78 mmol/L HA to the CP/Fe(II)/FA/CT process in a molar ratio of 12/6/12/1. The results also showed that the presence of HA enhanced the regeneration of Fe(II) from Fe(III), and the production of HO• increased one-fold when employing benzoic acid as the HO• probe. Additionally, FA slightly improves the production of HO•. A study of the mechanism confirmed that the carbon dioxide radical (CO2), a strong reductant generated by the reaction between FA and HO•, was the dominant radical responsible for CT degradation. Almost complete CT dechlorination was achieved in the process. The presence of humic acid and chloride ion slightly decreased CT removal, while high doses of bicarbonate and high pH inhibited CT degradation. This study helps us to better understand the synergistic roles of FA and HA for HO• and CO2 generation and the removal of perchlorinated hydrocarbons in modified Fenton systems.  相似文献   

8.
• The membrane bioreactor cost decreased by 38.2% by decreasing HRT from 72 h to 36 h. • Capital and operation costs contributed 62.1% and 37.9% to decreased costs. • The membrane bioreactor is 32.6% cheaper than the oxidation ditch for treatment. • The effluent COD also improved from 709.93±62.75 mg/L to 280±17.32 mg/L. • Further treatment also benefited from lower pretreatment investment. A cost sensitivity analysis was performed for an industrial membrane bioreactor to quantify the effects of hydraulic retention times and related operational parameters on cost. Different hydraulic retention times (72–24 h) were subjected to a flat-sheet membrane bioreactor updated from an existing 72 h oxidation ditch treating antibiotic production wastewater. Field experimental data from the membrane bioreactor, both full-scale (500 m3/d) and pilot (1.0 m3/d), were used to calculate the net present value (NPV), incorporating both capital expenditure (CAPEX) and operating expenditure. The results showed that the tank cost was estimated above membrane cost in the membrane bioreactor. The decreased hydraulic retention time from 72 to 36 h reduced the NPV by 38.2%, where capital expenditure contributed 24.2% more than operational expenditure. Tank construction cost was decisive in determining the net present value contributed 62.1% to the capital expenditure. The membrane bioreactor has the advantage of a longer lifespan flat-sheet membrane, while flux decline was tolerable. The antibiotics decreased to 1.87±0.33 mg/L in the MBR effluent. The upgrade to the membrane bioreactor also benefited further treatments by 10.1%–44.7% lower direct investment.  相似文献   

9.
• Real ML-GFW with high salinity and high organics was degraded by O3/H2O2 process. • Successful optimization of operation conditions was attained using RSM based on CCD. • Single-factor experiments in advance ensured optimal experimental conditions. • The satisfactory removal efficiency of TOC was achieved in spite of high salinity. • The initial pH plays the most significant role in the degradation of ML-GFW. The present study reports the use of the O3/H2O2 process in the pretreatment of the mother liquor of gas field wastewater (ML-GFW), obtained from the multi-effect distillation treatment of the gas field wastewater. The range of optimal operation conditions was obtained by single-factor experiments. Response surface methodology (RSM) based on the central composite design (CCD) was used for the optimization procedure. A regression model with Total organic carbon (TOC) removal efficiency as the response value was established (R2 = 0.9865). The three key factors were arranged according to their significance as: pH>H2O2 dosage>ozone flow rate. The model predicted that the best operation conditions could be obtained at a pH of 10.9, an ozone flow rate of 0.8 L/min, and H2O2 dosage of 6.2 mL. The dosing ratio of ozone was calculated to be 9.84 mg O3/mg TOC. The maximum removal efficiency predicted was 75.9%, while the measured value was 72.3%. The relative deviation was found to be in an acceptable range. The ozone utilization and free radical quenching experiments showed that the addition of H2O2 promoted the decomposition of ozone to produce hydroxyl radicals (·OH). This also improved the ozone utilization efficiency. Gas chromatography-mass spectrometry (GC-MS) analysis showed that most of the organic matters in ML-GFW were degraded, while some residuals needed further treatment. This study provided the data and the necessary technical supports for further research on the treatment of ML-GFW.  相似文献   

10.
• Pt/CZL exhibits the optimum catalytic performance for HC and NOx elimination. • The strong PM-Ce interaction favors the oxygen mobility and DOSC. • Pd/CZL shows higher catalytic activity for CO conversion due to more Olatt species. • Great oxygen mobility at high temperature broadens the dynamic operation window. • The relationship between DOSC and catalytic performance is revealed. The physicochemical properties of Pt-, Pd- and Rh- loaded (Ce,Zr,La)O2 (shorted for CZL) catalysts before/after aging treatment were systematically characterized by various techniques to illustrate the relationship of the dynamic oxygen storage/release capacity and redox ability with their catalytic performances for HC, NOx and CO conversions. Pt/CZL catalyst exhibits the optimum catalytic performance for HC and NOx elimination, which mainly contribute to its excellent redox ability and dynamic oxygen storage/release capacity (DOSC) at lower temperature due to the stronger PM (precious metals)-support interaction. However, the worse stability of Pt-O-Ce species and volatile Pt oxides easily result in the dramatical decline in catalytic activity after aging. Pd/CZL shows higher catalytic activity for CO conversion by reason of more Olatt species as the active oxygen for CO oxidation reaction. Rh/CZL catalyst displays the widest dynamic operation window for NOx elimination as a result of greater oxygen mobility at high temperature, and the ability to retain more Rh-O-Ce species after calcined at 1100°C effectively restrains sintering of active RhOx species, improving the thermal stability of Rh/CZL catalyst.  相似文献   

11.
• The calculation process and algorithm of response surface model (RSM) were enhanced. • The prediction errors of RSM in the margin and transition areas were greatly reduced. • The enhanced RSM was able to analyze O3-NOx-VOC sensitivity in real-time. • The O3 formations were mainly sensitive to VOC, for the two case study regions. Quantification of the nonlinearities between ambient ozone (O3) and the emissions of nitrogen oxides (NOx) and volatile organic compound (VOC) is a prerequisite for an effective O3 control strategy. An Enhanced polynomial functions Response Surface Model (Epf-RSM) with the capability to analyze O3-NOx-VOC sensitivities in real time was developed by integrating the hill-climbing adaptive method into the optimized Extended Response Surface Model (ERSM) system. The Epf-RSM could single out the best suited polynomial function for each grid cell to quantify the responses of O3 concentrations to precursor emission changes. Several comparisons between Epf-RSM and pf-ERSM (polynomial functions based ERSM) were performed using out-of-sample validation, together with comparisons of the spatial distribution and the Empirical Kinetic Modeling Approach diagrams. The comparison results showed that Epf-RSM effectively addressed the drawbacks of pf-ERSM with respect to over-fitting in the margin areas and high biases in the transition areas. The O3 concentrations predicted by Epf-RSM agreed well with Community Multi-scale Air Quality simulation results. The case study results in the Pearl River Delta and the north-western area of the Shandong province indicated that the O3 formations in the central areas of both the regions were more sensitive to anthropogenic VOC in January, April, and October, while more NOx-sensitive in July.  相似文献   

12.
• Quantitative global ARGs profile in dialysis water was investigated. • Totally 35 ARGs were found in the dialysis treatment train. • 29 ARGs (highest) were found in carbon filtration effluent. erm and mtrD-02 occurred in the final effluent. • The effluent was associated with health risks even after RO treatment. Dialysis water is directly related to the safety of hemodialysis patients, thus its quality is generally ensured by a stepwise water purification cascade. To study the effect of water treatment on the presence of antibiotic resistance genes (ARGs) in dialysis water, this study used propidium monoazide (PMA) in conjunction with high throughput quantitative PCR to analyze the diversity and abundance of ARGs found in viable bacteria from water having undergone various water treatment processes. The results indicated the presence of 35 ARGs in the effluents from the different water treatment steps. Twenty-nine ARGs were found in viable bacteria from the effluent following carbon filtration, the highest among all of the treatment processes, and at 6.96 Log (copies/L) the absolute abundance of the cphA gene was the highest. Two resistance genes, erm (36) and mtrD-02, which belong to the resistance categories macrolides-lincosamides-streptogramin B (MLSB) and other/efflux pump, respectively, were detected in the effluent following reverse osmosis treatment. Both of these genes have demonstrated the potential for horizontal gene transfer. These results indicated that the treated effluent from reverse osmosis, the final treatment step in dialysis-water production, was associated with potential health risks.  相似文献   

13.
• Metformin consumes O2−• and OH• induced by PM are proposed. • OH• dominated the oxidation of metformin compared with O2−• • Metformin can prevent the harm of ROS induced by PM to human health. • Antioxidative potential of metformin was first proposed to provide measures. Exposure to particulate matter (PM) can lead to the excessive accumulation of reactive oxygen species (ROS), which causes oxidative stress and endangers human health. In this study, the effects of metformin on PM-induced radicals were investigated, and the antioxidation reaction mechanism of metformin was analyzed by the density functional theory (DFT) method. The corresponding results revealed that the consumption rate of dithiothreitol (DTT) increased as the metformin concentration (0–40 mmol/L) increased under exposure to PM active components. Moreover, the OH radical content decreased as the metformin concentration increased. This result may be related to the consumption of PM-induced OH radicals by metformin, which promotes the DTT consumption rate. Additionally, because the initiation reaction has a high barrier, the oxidation reaction rate between metformin and •O2− is not very fast, although various catalysts may be present in the human environment. Importantly, we found that the barrier of metformin induced by OH radicals is only 9.6 kcal/mol while the barrier of metformin induced by oxygen is 57.9 kcal/mol, which shows that the rate of the •OH-initiated oxidative reaction of metformin is much faster and that this reaction path occurs more easily. By sample analysis, the mean OH radical generation was 55 nmol/min/g (ranging from 5 to 105 nmol/min/g) on haze days and 30 nmol/min/g (ranging from 10 to 50 nmol/min/g) on non-haze days. Moreover, OH radical generation was higher on haze days than on neighboring non-haze days. Taken together, all data suggest that metformin could consume the PM-induced radicals, such as OH radicals and •O2−, thereby providing health protection.  相似文献   

14.
• The SRAO phenomena tended to occur only under certain conditions. • High amount of biomass and non-anaerobic condition is requirement for SRAO. • Anammox bacteria cannot oxidize ammonium with sulfate as electron acceptor. • AOB and AnAOB are mainly responsible for ammonium conversion. • Heterotrophic sulfate reduction mainly contributed to sulfate conversion. For over two decades, sulfate reduction with ammonium oxidation (SRAO) had been reported from laboratory experiments. SRAO was considered an autotrophic process mediated by anammox bacteria, in which ammonium as electron donor was oxidized by the electron acceptor sulfate. This process had been attributed to observed transformations of nitrogenous and sulfurous compounds in natural environments. Results obtained differed largely for the conversion mole ratios (ammonium/sulfate), and even the intermediate and final products of sulfate reduction. Thus, the hypothesis of biological conversion pathways of ammonium and sulfate in anammox consortia is implausible. In this study, continuous reactor experiments (with working volume of 3.8L) and batch tests were conducted under normal anaerobic (0.2≤DO<0.5 mg/L) / strict anaerobic (DO<0.2 mg/L) conditions with different biomass proportions to verify the SRAO phenomena and identify possible pathways behind substrate conversion. Key findings were that SRAO occurred only in cases of high amounts of inoculant biomass under normal anaerobic condition, while absent under strict anaerobic conditions for same anammox consortia. Mass balance and stoichiometry were checked based on experimental results and the thermodynamics proposed by previous studies were critically discussed. Thus anammox bacteria do not possess the ability to oxidize ammonium with sulfate as electron acceptor and the assumed SRAO could, in fact, be a combination of aerobic ammonium oxidation, anammox and heterotrophic sulfate reduction processes.  相似文献   

15.
• Recent progress of As-contaminated soil remediation technologies is presented. • Phytoextraction and chemical immobilization are the most widely used methods. • Novel remediation technologies for As-contaminated soil are still urgently needed. • Methods for evaluating soil remediation efficiency are lacking. • Future research directions for As-contaminated soil remediation are proposed. Arsenic (As) is a top human carcinogen widely distributed in the environment. As-contaminated soil exists worldwide and poses a threat on human health through water/food consumption, inhalation, or skin contact. More than 200 million people are exposed to excessive As concentration through direct or indirect exposure to contaminated soil. Therefore, affordable and efficient technologies that control risks caused by excess As in soil must be developed. The presently available methods can be classified as chemical, physical, and biological. Combined utilization of multiple technologies is also common to improve remediation efficiency. This review presents the research progress on different remediation technologies for As-contaminated soil. For chemical methods, common soil washing or immobilization agents were summarized. Physical technologies were mainly discussed from the field scale. Phytoextraction, the most widely used technology for As-contaminated soil in China, was the main focus for bioremediation. Method development for evaluating soil remediation efficiency was also summarized. Further research directions were proposed based on literature analysis.  相似文献   

16.
• A V2O5/TiO2 granular catalyst for simultaneous removal of NO and chlorobenzene. • Catalyst synthesized by vanadyl acetylacetonate showed good activity and stability. • The kinetic model was established and the synergetic activity was predicted. • Both chlorobenzene oxidation and SCR of NO follow pseudo-first-order kinetics. • The work is of much value to design of multi-pollutants emission control system. The synergetic abatement of multi-pollutants is one of the development trends of flue gas pollution control technology, which is still in the initial stage and facing many challenges. We developed a V2O5/TiO2 granular catalyst and established the kinetic model for the simultaneous removal of NO and chlorobenzene (i.e., an important precursor of dioxins). The granular catalyst synthesized using vanadyl acetylacetonate precursor showed good synergistic catalytic performance and stability. Although the SCR reaction of NO and the oxidation reaction of chlorobenzene mutually inhibited, the reaction order of each reaction was not considerably affected, and the pseudo-first-order reaction kinetics was still followed. The performance prediction of this work is of much value to the understanding and reasonable design of a catalytic system for multi-pollutants (i.e., NO and dioxins) emission control.  相似文献   

17.
• A pilot study was conducted for drinking water treatment using loose NF membranes. • The membranes had very high rejection of NOM and medium rejection of Ca2+/Mg2+. • Organic fouling was dominant and contribution of inorganic fouling was substantial. • Both organic and inorganic fouling had spatial non-uniformity on membrane surface. • Applying EDTA at basic conditions was effective in removing membrane fouling. Nanofiltration (NF) using loose membranes has a high application potential for advanced treatment of drinking water by selectively removing contaminants from the water, while membrane fouling remains one of the biggest problems of the process. This paper reported a seven-month pilot study of using a loose NF membrane to treat a sand filtration effluent which had a relatively high turbidity (~0.4 NTU) and high concentrations of organic matter (up to 5 mg/L as TOC), hardness and sulfate. Results showed that the membrane demonstrated a high rejection of TOC (by>90%) and a moderately high rejection of two pesticides (54%–82%) while a moderate rejection of both calcium and magnesium (~45%) and a low rejection of total dissolved solids (~27%). The membrane elements suffered from severe membrane fouling, with the membrane permeance decreased by 70% after 85 days operation. The membrane fouling was dominated by organic fouling, while biological fouling was moderate. Inorganic fouling was mainly caused by deposition of aluminum-bearing substances. Though inorganic foulants were minor contents on membrane, their contribution to overall membrane fouling was substantial. Membrane fouling was not uniform on membrane. While contents of organic and inorganic foulants were the highest at the inlet and outlet region, respectively, the severity of membrane fouling increased from the inlet to the outlet region of membrane element with a difference higher than 30%. While alkaline cleaning was not effective in removing the membrane foulants, the use of ethylenediamine tetraacetate (EDTA) at alkaline conditions could effectively restore the membrane permeance.  相似文献   

18.
• Mechanism of DCM disproportionation over mesoporous TiO2 was studied. • DCM was completely eliminated at 350℃ under 1 vol.% humidity. • Anatase (001) was the key for disproportionation. • A competitive oxidation route co-existed with disproportionation. • Disproportionation was favored at low temperature. Mesoporous TiO2 was synthesized via nonhydrolytic template-mediated sol-gel route. Catalytic degradation performance upon dichloromethane over as-prepared mesoporous TiO2, pure anatase and rutile were investigated respectively. Disproportionation took place over as-made mesoporous TiO2 and pure anatase under the presence of water. The mechanism of disproportionation was studied by in situ FTIR. The interaction between chloromethoxy species and bridge coordinated methylenes was the key step of disproportionation. Formate species and methoxy groups would be formed and further turned into carbon monoxide and methyl chloride. Anatase (001) played an important role for disproportionation in that water could be dissociated into surface hydroxyl groups on such structure. As a result, the consumed hydroxyl groups would be replenished. In addition, there was another competitive oxidation route governed by free hydroxyl radicals. In this route, chloromethoxy groups would be oxidized into formate species by hydroxyl radicals transfering from the surface of TiO2. The latter route would be more favorable at higher temperature.  相似文献   

19.
• Submerged arc plasma was introduced in terms of wastewater treatment. • Ozone oxidation was coupled with submerged arc plasma system. • Ozone was converted into O and O2 by submerged arc plasma. • Decomposition rate was accelerated by submerged arc plasma. • Introduction of ozone led to significant increase in mineralization. Submerged arc plasma technology was assessed for the removal of phenols from wastewater. The OH radicals generated from the boundary between the plasma and waste solution were considered as a significant factor on the degradation reaction. In this study, the effects of highly energetic electrons released from the submerged arc plasma were mainly studied. The highly energetic electrons directly broke the strong chemical bond and locally increased the reaction temperatures in solution. The effects of the submerged-arc plasma on the decomposition of phenol are discussed in terms of the input energy and initial concentration. The single use of submerged arc plasma easily decomposed the phenol but did not increase the mineralization efficiency. Therefore, the submerged arc plasma, coupled with the ozone injection, was investigated. The submerged arc plasma combined with ozone injection had a synergic effect, which led to significant improvements in mineralization with only a small increase in input energy. The decomposition mechanism of phenol by the submerged arc plasma with the ozone was analyzed.  相似文献   

20.
• A novel and multi-functional clay-based oil spill remediation system was constructed. • TiO2@PAL functions as a particulate dispersant to break oil slick into tiny droplets. • Effective dispersion leads to the direct contact of TiO2 with oil pollutes directly. • TiO2 loaded on PAL exhibits efficient photodegradation for oil pollutants. • TiO2@PAL shows a typical dispersion-photocatalysis synergistic remediation. Removing spilled oil from the water surface is critically important given that oil spill accidents are a common occurrence. In this study, TiO2@Palygorskite composite prepared by a simple coprecipitation method was used for oil spill remediation via a dispersion-photodegradation synergy. Diesel could be efficiently dispersed into small oil droplets by TiO2@Palygorskite. These dispersed droplets had an average diameter of 20–30 mm and exhibited good time stability. The tight adsorption of TiO2@Palygorskite on the surface of the droplets was observed in fluorescence and SEM images. As a particulate dispersant, the direct contact of TiO2@Palygorskite with oil pollutants effectively enhanced the photodegradation efficiency of TiO2 for oil. During the photodegradation process, •O2and •OH were detected by ESR and radical trapping experiments. The photodegradation efficiency of diesel by TiO2@Palygorskite was enhanced by about 5 times compared with pure TiO2 under simulated sunlight irradiation. The establishment of this new dispersion-photodegradation synergistic remediation system provides a new direction for the development of marine oil spill remediation.  相似文献   

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